Supplemental Information

Molecular simulation of low temperature argon adsorption in several models of IRMOF-1 with defects and structural disorder

L. Sarkisov[a]

1. Forcefield parameters (Universal Force Field1)

Atom type / σ, Å / ε, K
C / 3.431 / 52.80
O / 3.118 / 30.20
H / 2.571 / 22.14
N / 3.261 / 34.70
Zn / 2.462 / 62.38
Ar / 3.440 / 93.27
Au / 2.934 / 19.61

2. Additional simulation details

Iterations, per adsorption point / 40·106 - 80·106
Cut-off (Å) / 12.8 (no tail corrections)
Type of moves / Insertion, deletion, translation, rotation (for non-spherical species)
Weight of each type of move / Equal weight
Iterations used for equilibration / 50%
Iterations used for statistical sampling / 50%
α and shield parameters for the Fennell-Gezelter method 2 / 0.1, 1.0
KMAX (number of unit cell images in the reciprocal space), κ (parameter related to the width of the Gaussian function, see http://www.iec.northwestern.edu/Music/
electrostatic/electrostatic.htm)
for the Ewald method / 15, 6.7
xyz dimensions of the system / 51.338, 51.338, 51.338
Angles of the unit cell (º) / 90.0, 90.0, 90.0

3. Additional details for constant temperature molecular dynamics of gold nanoclusters in IRMOF-1 at ambient temperature

Software / MuSiC3
Number of time steps / 10000000
Time step, ps / 0.0002
Integrator / Gear predictor-corrector
Thermostat / Nose-Hoover
Thermostat parameter, Qnose (kcal/mol) / 1000
Iterations used for statistical sampling / 50%
Temperature, K / 300

4. Structure of the Au13 cluster and partial charges from the Mulliken analysis4

Atom number / x / y / z / Type / q, e
1 / 0 / 0 / 0 / Au / -0.012
2 / 2.81675 / -0.06406 / -0.55608 / Au / -0.012
3 / 0.740504 / -0.35438 / -2.5232 / Au / 0.144
4 / 3.442945 / -0.49098 / -3.14435 / Au / -0.012
5 / 2.209357 / 1.941327 / -2.3734 / Au / -0.012
6 / -2.0049 / -0.2429 / -1.92655 / Au / -0.012
7 / -0.72809 / -2.65219 / -2.7371 / Au / -0.012
8 / 1.293648 / -2.43921 / -0.77963 / Au / -0.012
9 / -1.21937 / -0.62952 / -4.54356 / Au / -0.012
10 / 0.289067 / 1.682068 / -4.41479 / Au / -0.012
11 / -0.52443 / 2.085102 / -1.79024 / Au / -0.012
12 / 1.504473 / -0.7197 / -5.1262 / Au / -0.012
13 / 1.970518 / -2.81983 / -3.44875 / Au / -0.012

5. Structural characteristics of all systems, considered in this work

Reference perfect crystal / Percentage of the linkers removed / System with a 20Å mesopore / System with residual DMF / System with gold nanoclusters
5 / 10 / 20 / 50 / 65 / 73
Density g/cm3 / 0.604 / 0.593 / 0.581 / 0.558 / 0.481 / 0.423 / 0.287 / 0.428 / 0.625 / 0.762
Volume (He) cm3/g / 1.358 / 1.384 / 1.413 / 1.472 / 1.713 / 1.972 / 3.089 / 2.028 / 1.267 / 1.053
Surface area (m2/cm3) / 2043.91 / 2046.52 / 2066.93 / 2088.48 / 2137.96 / 2041.04 / 1457.04 / 1519.49 / 2026.6 / 2040.11
Surface area (m2/g) / 3381.49 / 3448.83 / 3556.78 / 3744.09 / 4446.09 / 4820.02 / 5084.12 / 3719.05 / 3242.3 / 2678.84
Pore limiting diameter (Å) / 7.71 / 7.71 / 7.71 / 7.71 / 8.84 / 9.93 / 16.63 / 21.41 / 7.52 / 7.65
Dmax (Å) / 14.95 / 14.95 / 14.95 / 14.95 / 16.84 / 19.4 / 25.67 / 24.58 / 14.71 / 14.85

1. A. K. Rappe, C. J. Casewit, K. S. Colwell, W. A. Goddard and W. M. Skiff, Journal of the American Chemical Society, 1992, 114, 10024-10035.

2. C. J. Fennell and J. D. Gezelter, Journal of Chemical Physics, 2006, 124.

3. A. Gupta, S. Chempath, M. J. Sanborn, L. A. Clark and R. Q. Snurr, Molecular Simulation, 2003, 29, 29-46.

4. X. Zhang, C. Q. Sun and H. Hirao, Physical Chemistry Chemical Physics, 2013, 15, 19284-19292.

2

[a] Institute for Materials and Processes, School of Engineering, The University of Edinburgh